WO2022198660A1 - Matériau d'ajout de lithium pour électrode positive et plaque d'électrode positive et dispositif électrochimique le comprenant - Google Patents
Matériau d'ajout de lithium pour électrode positive et plaque d'électrode positive et dispositif électrochimique le comprenant Download PDFInfo
- Publication number
- WO2022198660A1 WO2022198660A1 PCT/CN2021/083385 CN2021083385W WO2022198660A1 WO 2022198660 A1 WO2022198660 A1 WO 2022198660A1 CN 2021083385 W CN2021083385 W CN 2021083385W WO 2022198660 A1 WO2022198660 A1 WO 2022198660A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- positive electrode
- lithium
- supplement material
- present application
- lithium supplement
- Prior art date
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- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 128
- 239000000463 material Substances 0.000 title claims abstract description 99
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- 239000011159 matrix material Substances 0.000 claims abstract description 32
- 238000000034 method Methods 0.000 claims abstract description 28
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- 229910052742 iron Inorganic materials 0.000 claims abstract description 7
- 229910052759 nickel Inorganic materials 0.000 claims abstract description 7
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- 239000007774 positive electrode material Substances 0.000 claims description 19
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- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 description 1
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- DVATZODUVBMYHN-UHFFFAOYSA-K lithium;iron(2+);manganese(2+);phosphate Chemical compound [Li+].[Mn+2].[Fe+2].[O-]P([O-])([O-])=O DVATZODUVBMYHN-UHFFFAOYSA-K 0.000 description 1
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- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
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Images
Classifications
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- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/483—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides for non-aqueous cells
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
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- C—CHEMISTRY; METALLURGY
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- C01D—COMPOUNDS OF ALKALI METALS, i.e. LITHIUM, SODIUM, POTASSIUM, RUBIDIUM, CAESIUM, OR FRANCIUM
- C01D15/00—Lithium compounds
- C01D15/02—Oxides; Hydroxides
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G51/00—Compounds of cobalt
- C01G51/04—Oxides; Hydroxides
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G51/00—Compounds of cobalt
- C01G51/40—Cobaltates
- C01G51/42—Cobaltates containing alkali metals, e.g. LiCoO2
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/624—Electric conductive fillers
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- H—ELECTRICITY
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/628—Inhibitors, e.g. gassing inhibitors, corrosion inhibitors
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2002/00—Crystal-structural characteristics
- C01P2002/70—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data
- C01P2002/72—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data by d-values or two theta-values, e.g. as X-ray diagram
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2004/00—Particle morphology
- C01P2004/01—Particle morphology depicted by an image
- C01P2004/03—Particle morphology depicted by an image obtained by SEM
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2004/00—Particle morphology
- C01P2004/60—Particles characterised by their size
- C01P2004/61—Micrometer sized, i.e. from 1-100 micrometer
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/021—Physical characteristics, e.g. porosity, surface area
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/028—Positive electrodes
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Definitions
- the present application relates to the field of electrochemistry, and in particular, to a positive electrode lithium supplement material, a positive electrode pole piece comprising the material, and an electrochemical device.
- Lithium-ion secondary batteries have the advantages of high energy storage density, high open circuit voltage, low self-discharge rate, long cycle life, and good safety. They are widely used in various fields such as electrical energy storage, mobile electronic equipment, electric vehicles, and aerospace equipment. With the rapid development of mobile electronic devices and electric vehicles, the market has put forward higher and higher requirements for the energy density, cycle performance and kinetic performance of lithium-ion secondary batteries.
- Solid Electrolyte Interphase SEI
- SEI Solid Electrolyte Interphase
- the purpose of the present application is to provide a positive electrode lithium supplement material, a positive electrode electrode sheet and an electrochemical device comprising the material, so as to improve the energy density of the electrochemical device.
- the present application is explained by taking a lithium ion secondary battery as an example of the electrochemical device, but the electrochemical device of the present application is not limited to the lithium ion secondary battery.
- the specific technical solutions are as follows:
- a first aspect of the present application provides a positive electrode lithium supplement material, which includes a matrix of xLi 2 O ⁇ yM and carbon existing on the matrix; wherein x>0, 0.4x ⁇ y ⁇ 2x, and M includes Mn , at least one of Fe, Co, Ni, Cu, Cr or V.
- M may include at least one of Mn, Fe, Co, Ni, Cu, Cr, V, etc., and M may preferably include at least one of Mn, Fe, Co, Ni, and the like. Among them, the valence state of M can be 0.
- xLi 2 O.yM a matrix of xLi 2 O.yM that can achieve the purpose of the present application, such as but not limited to 4Li 2 O.3Co, Li 2 O.Co, Any of 5Li2O.4Co , 3Li2O.2Fe , 7Li2O.3Co.2Fe , 12Li2O.3Co.2Fe.2V , 2Li2O.Mn , Li2O.Ni , and the like.
- the xLi 2 O ⁇ yM matrix of the present application is obtained, which can release a large amount of lithium ions during the first charging process, has a high specific capacity, and can greatly improve the performance of lithium ion secondary batteries. Energy Density.
- the inventor unexpectedly found that the presence of carbon on the xLi 2 O yM matrix can not only effectively enhance the chemical stability of the xLi 2 O yM matrix, but also improve the stability of the positive electrode slurry, making it more difficult to agglomerate and more convenient for the positive electrode.
- the preparation and storage of the slurry and its coating on the positive electrode plate can improve the processability of the positive electrode slurry, and can also improve the energy density of the lithium ion secondary battery.
- the carbon existing on the substrate of xLi 2 O ⁇ yM can wrap the entire surface of the substrate or partially wrap the surface of the substrate.
- This application is not particularly limited, as long as the The purpose of the application is sufficient.
- the positive electrode lithium supplement material provided by the present application includes a matrix of xLi 2 O ⁇ yM and carbon existing on the matrix.
- the positive electrode lithium supplement material has high specific capacity, good chemical stability, moderate conductivity, and no gas is generated during the charging lithium supplement process, which can effectively improve the particle agglomeration phenomenon in the positive electrode slurry mixing process, and improve the positive electrode slurry. Processability. Adding the positive electrode lithium supplement material to the positive electrode plate can supplement the loss of active lithium caused by the generation of SEI, thereby further improving the energy density of the lithium ion secondary battery.
- the mass percentage content of carbon is 0.5% to 3% based on the total mass of the positive electrode lithium supplement material.
- the lower limit of the mass percentage of carbon can be included in the following values: 0.5% or 1%; the upper limit of the carbon mass percentage can be included in the following values: 2%, 2.5% or 3%.
- the mass percentage of carbon is too low (for example, less than 0.5%), it is difficult to enhance the chemical stability of the xLi 2 O yM matrix, and it is difficult to act as a barrier layer to separate the xLi 2 O yM matrix from the positive electrode.
- the mass percentage of carbon is too high (for example, higher than 3%), the impedance increases significantly, and the polarization increases with it, which seriously affects the actual specific capacity of the positive electrode lithium supplement material, which in turn affects the The effect of improving the energy density of lithium-ion secondary batteries.
- the mass percentage content of carbon in the positive electrode lithium supplement material within the above range, the stability of the positive electrode slurry can be effectively improved and the energy density of the lithium ion secondary battery can be improved.
- the first charge specific capacity of the positive electrode lithium supplement material is ⁇ 450 mAh/g. It shows that the specific capacity of the positive electrode lithium supplementary material is high, and a large amount of lithium ions can be released during the first charge to make up for the loss of active lithium caused by the formation of SEI, and enough lithium ions are inserted back into the positive electrode active material during the first discharge, which effectively improves the lithium ion
- the discharge specific capacity of the ion secondary battery improves the energy density of the lithium ion secondary battery.
- a second aspect of the present application provides a method for preparing the positive electrode lithium supplement material of the present application, comprising the following steps:
- a positive electrode lithium supplement material wherein, the molar ratio of naphthalene to lithium metal is 1: (0.6 to 1), and the molar ratio of naphthalene to oxide M a O b is 1 : (0.1 to 0.5), and the ratio of the mole number of naphthalene to the mass of the inorganic carbon source is 1: (0.05 to 0.3) mol/g.
- the above-mentioned preparation method provided in this application is a preferred method for preparing the positive electrode lithium supplementary material of the present application, and those skilled in the art can also prepare the positive electrode lithium supplementary material of the present application according to other methods. There is no special method for this application. Restrictions, as long as the purpose of the application can be achieved.
- the method for preparing a positive electrode lithium supplementary material provided by the present application is a homogeneous reaction at room temperature. Compared with the conventional solid-phase sintering method, the method has higher safety, more uniform and sufficient reaction, and the obtained product morphology and particles. Controllable.
- the preparation method is simple in principle, convenient in operation, excellent in effect, and has good compatibility with the existing preparation process.
- the type of solvent is not particularly limited, as long as the purpose of the present application can be achieved.
- it may be an aprotic solvent, including at least one of tetrahydrofuran, ethylene glycol dimethyl ether, and the like.
- the type of oxide M a O b is not particularly limited, as long as the purpose of the present application can be achieved.
- the oxide MaOb may include MnO , Mn2O3 , MnO2 , FeO , Fe2O3 , CoO , Co2O3 , Co3O4 , NiO , Ni2O3 , Cu2O , At least one of CuO, CrO, Cr 2 O 3 , CrO 3 , VO, V 2 O 3 , VO 2 or V 2 O 5 and the like.
- the inorganic carbon source may include at least one of carbon black, carbon gel, Ketjen black, acetylene black, carbon nanotubes, graphene, and the like.
- the temperature and time of calcination in step (4) are not particularly limited, as long as the purpose of the present application can be achieved.
- the calcination temperature may be 600°C to 700°C
- the calcination time may be 4h to 8h.
- a third aspect of the present application provides a positive electrode sheet, including a positive electrode lithium supplement material, and the positive electrode lithium supplement material is the positive electrode lithium supplement material described in any one of the above embodiments.
- the application of the positive electrode lithium supplement material of the present application to the positive electrode plate can realize the effective supplement of active lithium and improve the energy density of the lithium ion secondary battery.
- the positive electrode sheet in the present application is not particularly limited, as long as the purpose of the present application can be achieved.
- a positive electrode sheet typically includes a positive electrode current collector and a positive electrode active material layer.
- the positive electrode current collector is not particularly limited, as long as the purpose of the present application can be achieved, for example, it may include aluminum foil, aluminum alloy foil, or composite current collector.
- the positive electrode active material layer includes a positive electrode active material and a positive electrode lithium supplement material.
- the type of positive active material is not particularly limited, as long as it can achieve the purpose of the present application, for example, it can include nickel cobalt lithium manganate (811, 622, 523, 111), nickel cobalt lithium aluminate, lithium iron phosphate, lithium rich manganese At least one of base material, lithium cobaltate, lithium manganate, lithium iron manganese phosphate or lithium titanate.
- the positive electrode lithium supplement material is at least one of the positive electrode lithium supplement materials provided in this application.
- the thicknesses of the positive electrode current collector and the positive electrode active material layer are not particularly limited as long as the purpose of the present application can be achieved.
- the thickness of the positive electrode current collector is 5 ⁇ m to 20 ⁇ m, preferably 6 ⁇ m to 18 ⁇ m, and more preferably 8 ⁇ m to 16 ⁇ m.
- the thickness of the positive electrode material layer is 30 ⁇ m to 120 ⁇ m.
- the positive electrode active material layer may be provided on one surface (the first surface) of the positive electrode current collector in the thickness direction, or may be provided on both surfaces (the first surface and the second surface) in the thickness direction of the positive electrode current collector )superior.
- the “surface” here can be the entire area of the positive electrode current collector, or a partial area of the positive electrode current collector, which is not particularly limited in this application, as long as the purpose of the application can be achieved.
- the positive electrode sheet may further comprise a conductive layer, and the conductive layer is located between the positive electrode current collector and the positive electrode material layer.
- the composition of the conductive layer is not particularly limited, and may be a conductive layer commonly used in the art.
- the conductive layer includes a conductive agent and a binder.
- the mass percentage content of the positive electrode lithium supplement material may be 1% to 10%, preferably 3% to 10%.
- the mass percentage content of the positive electrode lithium supplement material may include: 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, 10%, and the like.
- the positive electrode lithium supplement material may be directly added to the slurry during the positive electrode material slurry mixing process to form a positive electrode slurry containing the positive electrode lithium supplement material of the present application, which is coated on the surface of the positive electrode current collector. It is also possible to pre-deposit a positive electrode lithium supplement material film on the surface of the positive electrode current collector. It is also possible to deposit a positive electrode lithium supplement material film on the surface of the positive electrode active material after the positive electrode active material of the positive electrode sheet is coated.
- the lithium ion secondary battery is assembled after the positive electrode lithium supplement material is added. During the first charging process, the positive electrode lithium supplement material is delithiated and the lithium supplement effect can be exerted.
- the above-mentioned "surface" may be the entire area of the positive electrode current collector/positive electrode active material, or may be a partial area of the positive electrode current collector/positive electrode active material, which is not particularly limited in this application, as long as the purpose of the application can be achieved. Can.
- the negative electrode sheet of the present application is not particularly limited, as long as the purpose of the present application can be achieved.
- a negative electrode sheet typically includes a negative electrode current collector and a negative electrode active material layer.
- the negative electrode current collector is not particularly limited as long as it can achieve the purpose of the present application.
- the anode active material layer includes an anode active material, a conductive agent, and a thickener.
- the negative electrode active material of the present application may include natural graphite, artificial graphite, mesophase microcarbon beads (MCMB), hard carbon, soft carbon, silicon, silicon-carbon composite, SiO x (0 ⁇ x ⁇ 2), Li-Sn At least one of alloys, Li-Sn-O alloys, Sn, SnO, SnO 2 , spinel-structured lithium titanate Li 4 Ti 5 O 12 , Li-Al alloys, metallic lithium, and the like.
- MCMB mesophase microcarbon beads
- the thickness of the negative electrode current collector and the negative electrode active material layer is not particularly limited, as long as the purpose of the present application can be achieved, for example, the thickness of the negative electrode current collector is 6 ⁇ m to 10 ⁇ m, and the thickness of the negative electrode active material layer is 30 ⁇ m to 120 ⁇ m.
- the thickness of the negative electrode sheet is not particularly limited, as long as the purpose of the present application can be achieved, for example, the thickness of the negative electrode sheet is 50 ⁇ m to 150 ⁇ m.
- the negative electrode sheet may further comprise a conductive layer, and the conductive layer is located between the negative electrode current collector and the negative electrode material layer.
- the composition of the conductive layer is not particularly limited, and may be a conductive layer commonly used in the art.
- the conductive layer includes a conductive agent and a binder.
- the conductive agent is not particularly limited as long as the object of the present application can be achieved.
- the conductive agent may include conductive carbon black (Super P), carbon nanotubes (CNTs), carbon nanofibers, flake graphite, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, or graphene, among others. at least one.
- the above-mentioned binder is not particularly limited, and any binder known in the art can be used as long as the purpose of the present application can be achieved.
- the binder may include polyacryl alcohol, sodium polyacrylate, potassium polyacrylate, lithium polyacrylate, polyimide, polyimide, polyamideimide, styrene butadiene rubber (SBR), polyvinyl alcohol ( PVA), polyvinylidene fluoride, polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), polyvinyl butyral (PVB), water-based acrylic resin, carboxymethyl cellulose (CMC) or carboxymethyl At least one of sodium cellulose (CMC-Na) and the like.
- SBR styrene butadiene rubber
- PVA polyvinyl alcohol
- PVDF polyvinylidene fluoride
- PVDF polyvinylidene fluoride
- PTFE polytetrafluoroethylene
- PVB polyvinyl butyral
- water-based acrylic resin carboxymethyl cellulose (CMC) or carboxymethyl At least one of sodium cellulose (CMC-Na)
- the separator in the present application is not particularly limited as long as the purpose of the present application can be achieved.
- polyethylene (PE), polypropylene (PP)-based polyolefin (PO) separators polyester films (such as polyethylene terephthalate (PET) films), cellulose films, polyimide Amine film (PI), polyamide film (PA), spandex or aramid film, woven film, non-woven film (non-woven fabric), microporous film, composite film, diaphragm paper, rolled film, spinning film, etc. at least one of.
- the release film may include a substrate layer and a surface treatment layer.
- the substrate layer can be a non-woven fabric, film or composite film with a porous structure, and the material of the substrate layer can include at least one of polyethylene, polypropylene, polyethylene terephthalate, polyimide, etc. kind.
- polypropylene porous membranes, polyethylene porous membranes, polypropylene non-woven fabrics, polyethylene non-woven fabrics, or polypropylene-polyethylene-polypropylene porous composite membranes may be used.
- at least one surface of the substrate layer is provided with a surface treatment layer, and the surface treatment layer can be a polymer layer or an inorganic layer, or a layer formed by mixing a polymer and an inorganic substance.
- the inorganic layer includes inorganic particles and a binder
- the inorganic particles are not particularly limited, and can be selected from aluminum oxide, silicon oxide, magnesium oxide, titanium oxide, hafnium dioxide, tin oxide, ceria, nickel oxide, for example , at least one of zinc oxide, calcium oxide, zirconium oxide, yttrium oxide, silicon carbide, boehmite, aluminum hydroxide, magnesium hydroxide, calcium hydroxide and barium sulfate.
- the binder is not particularly limited, for example, it can be selected from polyvinylidene fluoride, vinylidene fluoride-hexafluoropropylene copolymer, polyamide, polyacrylonitrile, polyacrylate, polyacrylic acid, polyacrylate, polyethylene One or a combination of rolidone, polyvinyl ether, polymethyl methacrylate, polytetrafluoroethylene and polyhexafluoropropylene.
- the polymer layer contains a polymer, and the material of the polymer includes polyamide, polyacrylonitrile, acrylate polymer, polyacrylic acid, polyacrylate, polyvinylpyrrolidone, polyvinyl ether, polyvinylidene fluoride or poly( At least one of vinylidene fluoride-hexafluoropropylene) and the like.
- the lithium ion secondary battery of the present application further includes an electrolyte, and the electrolyte may be at least one of a gel electrolyte, a solid electrolyte, and an electrolytic solution, and the electrolytic solution includes a lithium salt and a non-aqueous solvent.
- the lithium salt may include LiPF 6 , LiBF 4 , LiAsF 6 , LiClO 4 , LiB(C 6 H 5 ) 4 , LiCH 3 SO 3 , LiCF 3 SO 3 , LiN(SO 2 CF 3 ) 2. At least one of LiC(SO 2 CF 3 ) 3 , LiSiF 6 , LiBOB or lithium difluoroborate.
- LiPF 6 may be chosen as the lithium salt because it gives high ionic conductivity and improves cycling characteristics.
- the non-aqueous solvent may be a carbonate compound, a carboxylate compound, an ether compound, other organic solvents, or a combination thereof.
- the above-mentioned carbonate compound may be a chain carbonate compound, a cyclic carbonate compound, a fluorocarbonate compound, or a combination thereof.
- Examples of the above-mentioned chain carbonate compound are dimethyl carbonate (DMC), diethyl carbonate (DEC), dipropyl carbonate (DPC), methylpropyl carbonate (MPC), ethylpropyl carbonate (EPC), carbonic acid Methyl ethyl ester (MEC) and combinations thereof.
- Examples of cyclic carbonate compounds are ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate (BC), vinylethylene carbonate (VEC), and combinations thereof.
- fluorocarbonate compounds are fluoroethylene carbonate (FEC), 1,2-difluoroethylene carbonate, 1,1-difluoroethylene carbonate, 1,1,2-trifluoroethylene carbonate Ethyl carbonate, 1,1,2,2-tetrafluoroethylene carbonate, 1-fluoro-2-methylethylene carbonate, 1-fluoro-1-methylethylene carbonate, 1,2-dicarbonate Fluoro-1-methylethylene, 1,1,2-trifluoro-2-methylethylene carbonate, trifluoromethylethylene carbonate, and combinations thereof.
- FEC fluoroethylene carbonate
- 1,2-difluoroethylene carbonate 1,1-difluoroethylene carbonate
- 1,1,2-trifluoroethylene carbonate Ethyl carbonate 1,1,2,2-tetrafluoroethylene carbonate
- 1-fluoro-2-methylethylene carbonate 1-fluoro-1-methylethylene carbonate
- 1,2-dicarbonate Fluoro-1-methylethylene 1,1,2-trifluoro-2-methylethylene carbonate, trifluoromethyl
- carboxylate compounds are methyl formate, methyl acetate, ethyl acetate, n-propyl acetate, tert-butyl acetate, methyl propionate, ethyl propionate, propyl propionate, ⁇ -butyrolactone , caprolactone, valerolactone, mevalonolactone, caprolactone, and combinations thereof.
- ether compounds examples include dibutyl ether, tetraglyme, diglyme, 1,2-dimethoxyethane, 1,2-diethoxyethane, ethoxymethyl ether Oxyethane, 2-methyltetrahydrofuran, tetrahydrofuran, and combinations thereof.
- Examples of the above-mentioned other organic solvents are dimethyl sulfoxide, 1,2-dioxolane, sulfolane, methyl sulfolane, 1,3-dimethyl-2-imidazolidinone, N-methyl-2-pyrrolidone, Formamide, dimethylformamide, acetonitrile, trimethyl phosphate, triethyl phosphate, trioctyl phosphate, and phosphate esters and combinations thereof.
- a fourth aspect of the present application provides an electrochemical device including the positive electrode plate provided by the present application, and the electrochemical device has good energy density.
- the electrochemical device of the present application is not particularly limited, and it may include any device in which an electrochemical reaction occurs.
- the electrochemical device may include, but is not limited to, a lithium metal secondary battery, a lithium ion secondary battery (lithium ion battery), a lithium polymer secondary battery, or a lithium ion polymer secondary battery, and the like.
- the present application also provides an electronic device comprising the electrochemical device described in the embodiments of the present application, and the electronic device has good energy density.
- the electronic device of the present application is not particularly limited, and it may be used for any electronic device known in the prior art.
- electronic devices may include, but are not limited to, notebook computers, pen input computers, mobile computers, e-book players, portable telephones, portable fax machines, portable copiers, portable printers, headsets, VCRs, LCD TVs, portable cleaners, portable CD players, mini discs, transceivers, electronic notepads, calculators, memory cards, portable recorders, radios, backup power supplies, motors, automobiles, motorcycles, assisted bicycles, bicycles, Lighting equipment, toys, game consoles, clocks, power tools, flashlights, cameras, large-scale household storage batteries and lithium-ion capacitors, etc.
- an electrochemical device can be manufactured by the following process: overlapping the positive electrode and the negative electrode through a separator, wrapping them, folding them, etc., and putting them into the casing as needed, injecting the electrolyte into the casing and sealing it, wherein
- the separator used is the aforementioned separator provided in this application.
- an overcurrent preventing element, a guide plate, etc. may be placed in the case to prevent pressure rise and overcharge and discharge inside the electrochemical device.
- the present application provides a positive electrode lithium supplement material, a positive electrode electrode sheet comprising the material, and an electrochemical device.
- the positive electrode lithium supplement material includes: a matrix of xLi 2 O ⁇ yM, and carbon existing on the matrix; wherein, x >0, 0.4x ⁇ y ⁇ 2x, M includes at least one of Mn, Fe, Co, Ni, Cu, Cr or V.
- the positive electrode lithium supplement material has strong chemical stability, and can effectively improve the particle agglomeration phenomenon in the slurry mixing process. Applying the positive electrode lithium supplement material in the positive electrode plate can realize the supplement of active lithium and effectively improve the energy density of the electrochemical device.
- Fig. 1 is the XRD (X-ray diffraction) pattern of the positive electrode lithium supplement material of Example 1 of the application;
- Fig. 2 is the SEM (scanning electron microscope) image of the positive electrode lithium supplement material of Example 1 of the application;
- Fig. 3 is the cobalt element EDS (X-ray energy dispersive analysis) spectrum in the positive electrode lithium supplement material of Example 1 of the application;
- Fig. 4 is the oxygen element EDS spectrum in the positive electrode lithium supplement material of Example 1 of the application;
- FIG. 5 is an EDS spectrum of carbon element in the positive electrode lithium supplement material of Example 1 of the present application.
- the present application is explained by taking a lithium ion secondary battery as an example of an electrochemical device, but the electrochemical device of the present application is not limited to a lithium ion secondary battery.
- FIG. 1 shows the XRD pattern of the positive electrode lithium supplement material of Example 1 of the present application.
- (a) in FIG. 1 is the spectrum of the positive electrode lithium supplement material
- (b) in FIG. 1 is a Co standard diffraction card
- (c) in FIG. 1 is a Li 2 O standard diffraction card.
- FIG. 2 shows a SEM image of the positive electrode lithium supplement material of Example 1 of the present application. As shown in FIG. 2 , the particle size distribution of the positive electrode lithium supplement material is uniform.
- 3 shows the EDS spectrum of cobalt element in the positive electrode lithium supplement material of Example 1 of the present application, indicating that the positive electrode lithium supplement material of the present application contains cobalt element and is uniformly distributed in the positive electrode lithium supplement material.
- FIG. 4 shows the EDS spectrum of oxygen element in the positive electrode lithium supplement material of Example 1 of the present application, indicating that the positive electrode lithium supplement material of the present application contains oxygen element and is uniformly distributed in the positive electrode lithium supplement material.
- 5 shows the EDS spectrum of carbon element in the positive electrode lithium supplement material of Example 1 of the present application, indicating that the positive electrode lithium supplement material of the present application contains carbon element and is uniformly distributed in the positive electrode lithium supplement material.
- the positive electrode lithium supplement material to be tested, the conductive agent conductive carbon black (Super P) and the binder polyvinylidene fluoride (PVDF) were mixed in a mass ratio of 80:10:10, and N-methylpyrrolidone (NMP) was added as The solvent was mixed and prepared into a slurry with a solid content of 40%, and a coating of 100 ⁇ m thickness was applied on the current collector aluminum foil with a scraper. A 1cm-diameter disk was formed, a metal lithium sheet was used as a counter electrode in a glove box, a ceglard composite membrane was selected as the separator, and an electrolyte solution was added to assemble to obtain a button battery.
- Super P conductive agent conductive carbon black
- PVDF binder polyvinylidene fluoride
- NMP N-methylpyrrolidone
- the electrolyte is ethylene carbonate (EC), ethyl methyl carbonate (EMC) and diethyl carbonate (DEC) in a mass ratio of 30:50:20 to obtain an organic solution, and then add lithium salt lithium hexafluorophosphate to the organic solvent to dissolve and mix uniform, and an electrolyte solution with a lithium salt concentration of 1.15 mol/L was obtained.
- EC ethylene carbonate
- EMC ethyl methyl carbonate
- DEC diethyl carbonate
- Wuhan Blue Electric CT2001A system is used to test the specific charging capacity.
- the button-type battery to be tested containing the positive electrode lithium supplementary material is allowed to stand for 30min in the environment of 25 ⁇ 3°C, and the rate of 0.1C (the theoretical gram of the positive electrode lithium supplementary material)
- the capacity was calculated at 600mAh/g) with constant current charging to a voltage of 4.45V, followed by constant voltage charging to a current of 0.025C, and the first charging capacity was recorded.
- the charging specific capacity of the button battery of the positive electrode lithium supplement material the first charging capacity/the quality of the positive electrode lithium supplement material.
- the lithium ion secondary battery to be tested containing the positive electrode lithium supplement material was left standing for 30min in the environment of 25 ⁇ 3°C, charged with a constant current of 600mA (rated capacity in 2000mAh) to a voltage of 4.4V, and then charged with a constant voltage to 4.4V.
- the current was 50mA, and it was allowed to stand for 5min, and the discharge capacity was recorded for the first time by constant current discharge at a current of 600mA to a termination voltage of 3.0V.
- the positive electrode active material lithium cobalt oxide (LiCoO 2 ), the positive electrode lithium supplement material prepared above, the conductive agent Super P, and the binder PVDF are mixed according to the mass ratio of 95:2:1.5:1.5, and NMP is added as a solvent.
- the slurry was uniformly coated on one surface of a positive electrode current collector aluminum foil with a thickness of 10 ⁇ m, and dried at 130° C. to obtain a positive electrode sheet with a coating thickness of 110 ⁇ m.
- the single-side coating of the positive electrode sheet is completed.
- the above steps are repeated on the other surface of the positive electrode sheet to obtain a positive electrode sheet coated with positive active material on both sides.
- the positive pole piece is cut into a size of 74mm ⁇ 867mm, and the tabs are welded for use.
- the graphite, the negative electrode active material SiO, the conductive agent nano-conductive carbon black, and the binder polyacryl alcohol (PAA) were mixed according to the mass ratio of 78:15:3:4, and deionized water was added as a solvent to prepare a solid content of 60 % slurry, and stir evenly, then add an appropriate amount of deionized water, adjust the viscosity of the slurry to 5000 Pa ⁇ s, and prepare a negative electrode slurry.
- the slurry was uniformly coated on the negative current collector copper foil with a thickness of 8 ⁇ m, dried at 110°C, and cold pressed to obtain a single-sided negative electrode sheet with an active material layer coated with an active material layer with a thickness of 100 ⁇ m.
- these steps are also completed on the back side of the negative electrode pole piece by the same method, that is, the negative pole piece with double-sided coating is obtained.
- the negative pole piece is cut into a size of 76mm ⁇ 851mm, and the tabs are welded for use.
- organic solvents EC, EMC and DEC were mixed in a mass ratio of 30:50:20 to obtain an organic solution, and then a lithium salt lithium hexafluorophosphate was added to the organic solvent to dissolve and mix evenly to obtain a lithium salt concentration of 1.15mol /L of electrolyte.
- a polypropylene (PP) film (supplied by Celgard) with a thickness of 14 ⁇ m was used.
- the positive electrode, the separator and the negative electrode prepared above are stacked in sequence, so that the separator is placed between the positive and negative electrodes to play a role of isolation, and the electrode assembly is obtained by winding.
- the electrode assembly is put into an aluminum-plastic film packaging bag, and the moisture is removed at 80°C, and the prepared electrolyte is injected.
- Example 15 ⁇ preparation of positive electrode lithium supplement material>, ⁇ preparation of positive electrode pole piece>, ⁇ preparation of negative electrode pole piece>, ⁇ preparation of electrolyte>, ⁇ preparation of separator> and The preparation steps of ⁇ Preparation of Lithium Ion Secondary Battery> are the same as those in Example 1, and the changes of relevant preparation parameters are shown in Table 1:
- the negative electrode active material graphite, nano-conductive carbon black, styrene-butadiene rubber and sodium carboxymethyl cellulose are mixed according to the mass ratio of 95:2:2:1, and deionized water is added as a solvent to prepare a slurry with a solid content of 70%. ingredients and mix well.
- the slurry was uniformly coated on the negative current collector copper foil with a thickness of 8 ⁇ m, dried at 110° C., and cold pressed to obtain a negative electrode pole piece with an active material layer of 150 ⁇ m in thickness on one side coated with an active material layer.
- these steps are also completed on the back side of the negative electrode pole piece by the same method, that is, the negative pole piece with double-sided coating is obtained.
- the negative pole piece is cut into a size of 76mm ⁇ 851mm, and the tabs are welded for use.
- Comparative Example 1 Comparative Example 2, Comparative Example 3 and Comparative Example 4, ⁇ Preparation of Positive Electrode Sheet>, ⁇ Preparation of Negative Electrode Sheet>, ⁇ Preparation of Electrolyte>, ⁇ Preparation of Separator> and ⁇ Lithium Ion Preparation of secondary battery>
- the preparation steps are the same as in Example 1.
- Comparative Example 2 Comparative Example 3 and Comparative Example 4, ⁇ Preparation of positive electrode lithium supplement material> is the same as Example 1, and the changes in relevant preparation parameters are as follows: As shown in Table 2:
- Example 1 Example 2, Example 3, Example 4, Example 5, Example 6, Example 7, Example 8, Example 9, Example 10, Example 11, Example 12, Example 13.
- the preparation parameters of Example 14, Example 15, Example 16, Example 17, Comparative Example 1, Comparative Example 2, Comparative Example 3, Comparative Example 4, and Comparative Example 5 are shown in Table 3:
- Example 1 Example 6, Example 7, Example 8, Example 9, Example 10, Example 11, Example 12 and Comparative Example 1 and Comparative Example 5 that the same components and The content of the inorganic carbon source wraps the matrix with different components to form different cathode lithium supplement materials.
- the composition of the matrix is different, as long as the composition of the matrix is within the scope of the present application, the chemical stability of the positive electrode lithium supplement material can be effectively improved, and the particle agglomeration phenomenon during the slurry mixing process of the positive electrode can be effectively suppressed.
- the application of the above-mentioned positive electrode lithium supplement material in the positive electrode plate can effectively supplement the active lithium, so that the energy density of the lithium ion secondary battery can be effectively improved.
- Example 1 Example 2, Example 3 and Comparative Example 2 and Comparative Example 3 that the positive electrode lithium supplementary material with the carbon content of the present application can effectively improve the first charge specific capacity of the positive electrode lithium supplementary material, and can achieve The active lithium is effectively supplemented, so that the energy density of the lithium-ion secondary battery is effectively improved.
- the calcination temperature, calcination time and the type of inorganic carbon source of the positive electrode lithium supplement material usually also affect the first charge specific capacity of the positive electrode lithium supplement material. It can be seen from Examples 1, 4 and 5 that as long as the above preparation is used If the parameters are within the scope of the present application, the first charge specific capacity of the positive electrode lithium supplementary material and the energy density of the lithium ion secondary battery can be effectively improved.
- Example 1 Example 13, Example 14, Example 15, Example 16 and Comparative Example 4 that the content of the positive electrode lithium supplementary material is within the scope of the application, which can effectively improve the first charge of the positive electrode lithium supplementary material Specific capacity and energy density of lithium-ion secondary batteries.
- the mass percentage of the positive electrode lithium supplement material is preferably 3% to 10%, for example, Example 13, Example 14, Example 15, Example 16, can more effectively improve the energy of the lithium ion secondary battery density.
- the cathode lithium supplement material provided by the present application includes a matrix of xLi 2 O ⁇ yM and carbon existing on the matrix.
- the positive electrode lithium supplement material has strong chemical stability, and can effectively improve the particle agglomeration phenomenon in the slurry mixing process. Applying the cathode lithium supplement material to an electrochemical device can effectively supplement active lithium and effectively improve the energy density of the electrochemical device.
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Abstract
La présente invention concerne un matériau d'ajout de lithium pour électrode positive, et une plaque d'électrode positive et un dispositif électrochimique le comprenant. Le matériau d'ajout de lithium pour électrode positive comprend : une matrice xLi2O•yM et du carbone présent sur la matrice, avec x > 0, 0,4x ≤ y ≤ 2x et M comprenant au moins un élément parmi Mn, Fe, Co, Ni, Cu, Cr ou V. Le matériau d'ajout de lithium pour électrode positive présente une grande stabilité chimique et peut améliorer efficacement le phénomène d'agrégation de particules pendant un processus de mélange de pâte. Le matériau d'ajout de lithium pour électrode positive est appliqué à la plaque d'électrode positive, de façon à pouvoir ajouter du lithium actif, et à pouvoir améliorer efficacement la densité d'énergie du dispositif électrochimique.
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